WO2014157418A1 - 非水電解質二次電池 - Google Patents

非水電解質二次電池 Download PDF

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Publication number
WO2014157418A1
WO2014157418A1 PCT/JP2014/058686 JP2014058686W WO2014157418A1 WO 2014157418 A1 WO2014157418 A1 WO 2014157418A1 JP 2014058686 W JP2014058686 W JP 2014058686W WO 2014157418 A1 WO2014157418 A1 WO 2014157418A1
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Prior art keywords
negative electrode
active material
electrode active
material layer
battery
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PCT/JP2014/058686
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English (en)
French (fr)
Japanese (ja)
Inventor
小川　弘志
本田　崇
康介 萩山
隆太 山口
Original Assignee
日産自動車株式会社
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Application filed by 日産自動車株式会社 filed Critical 日産自動車株式会社
Priority to CN201480018564.6A priority Critical patent/CN105074999B/zh
Priority to KR1020157026749A priority patent/KR101634919B1/ko
Priority to JP2015508633A priority patent/JP6004088B2/ja
Priority to EP14775855.1A priority patent/EP2983235B1/en
Priority to US14/779,912 priority patent/US20160064737A1/en
Publication of WO2014157418A1 publication Critical patent/WO2014157418A1/ja

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/60—Other road transportation technologies with climate change mitigation effect
    • Y02T10/70—Energy storage systems for electromobility, e.g. batteries

Definitions

  • the present invention relates to a non-aqueous electrolyte secondary battery.
  • a secondary battery that can be repeatedly charged and discharged is suitable as a power source for driving these motors, and a non-aqueous electrolyte secondary battery such as a lithium ion secondary battery that can be expected to have a high capacity and a high output is attracting attention.
  • a non-aqueous electrolyte secondary battery generally includes a positive electrode having a positive electrode active material layer containing a positive electrode active material (for example, a lithium-transition metal composite oxide) and a negative electrode active material (for example, a carbonaceous material such as graphite). And a negative electrode having a negative electrode active material layer including a battery element laminated with a separator interposed therebetween.
  • a positive electrode active material for example, a lithium-transition metal composite oxide
  • a negative electrode active material for example, a carbonaceous material such as graphite
  • the binder for binding the active material used in the active material layer is an organic solvent binder (a binder that does not dissolve / disperse in water but dissolves / disperses in an organic solvent) and an aqueous binder (a binder that dissolves / disperses in water). )are categorized.
  • the organic solvent-based binder requires a large amount of cost for materials, recovery, and disposal of the organic solvent, which may be industrially disadvantageous.
  • water-based binders make it easy to procure water as a raw material, and since steam is generated during drying, capital investment in the production line can be greatly suppressed, and the environmental burden is reduced. There is an advantage that you can. Further, the water-based binder has an advantage that the binding effect is large even in a small amount compared to the organic solvent-based binder, the active material ratio per volume can be increased, and the capacity of the negative electrode can be increased.
  • Patent Document 1 discloses that a negative electrode current collector and a negative electrode active material layer are used by combining different types of aqueous binders in a negative electrode active material layer of a nonaqueous electrolyte secondary battery. A method for improving adhesion (peel strength) is disclosed.
  • an object of the present invention is to provide a non-aqueous electrolyte secondary battery having high vibration resistance when an aqueous binder is used as a binder for a negative electrode active material layer.
  • the present inventors have conducted intensive research to solve the above problems.
  • the ratio of the length of the negative electrode active material layer to the long side is set to 1.25 or less, and the amount of the aqueous binder in the negative electrode active material layer is set to a predetermined value.
  • the present inventors have found that the above-mentioned problems can be solved by controlling to the above range, and have completed the present invention.
  • the present invention provides a power generation element including a positive electrode in which a positive electrode active material layer is formed on the surface of a positive electrode current collector, a negative electrode in which a negative electrode active material layer is formed on the surface of a negative electrode current collector, and a separator.
  • a non-aqueous electrolyte secondary battery having a flat plate structure, wherein the negative electrode active material layer contains 2 to 4% by mass of an aqueous binder with respect to the total mass of the negative electrode active material layer, and the negative electrode active material layer Is a non-aqueous electrolyte secondary battery in which the ratio of the long side to the short side of the rectangle is 1 to 1.25.
  • 1 is a schematic cross-sectional view showing a basic configuration of a non-aqueous electrolyte lithium ion secondary battery that is an embodiment of the present invention and is not a flat (stacked) bipolar type. It is the schematic of the negative electrode used for the nonaqueous electrolyte secondary battery of this embodiment. 1 is a plan view of a nonaqueous electrolyte secondary battery which is a preferred embodiment of the present invention. It is an arrow view from A of FIG. 3A.
  • the present invention provides a power generation element including a positive electrode in which a positive electrode active material layer is formed on the surface of a positive electrode current collector, a negative electrode in which a negative electrode active material layer is formed on the surface of a negative electrode current collector, and a separator.
  • a non-aqueous electrolyte secondary battery of a flat plate type wherein the negative electrode active material layer contains 2 to 4% by mass of an aqueous binder with respect to the total mass of the negative electrode active material layer, and the negative electrode active material layer comprises A non-aqueous electrolyte secondary battery having a rectangular shape and having a length ratio (long side / short side) of the long side to the short side of the rectangle of 1 to 1.25.
  • the current collector follows the expansion / contraction of the negative electrode active material layer, residual stress hardly occurs, and the electrode has a shape close to a square. It is easy to release stress around. Moreover, high binding property is securable by making content of an aqueous binder into a specific value. Therefore, the peel strength between the negative electrode current collector and the negative electrode active material layer is improved, and a battery having high vibration resistance can be obtained.
  • water-based binders can use water as a solvent for producing an active material layer, so there are various advantages, and the active material is bound in a smaller amount than organic solvent-based binders. Can be made.
  • non-aqueous electrolyte secondary batteries used as power sources for driving motors in vehicles are given strong vibrations, they are more resistant to vibration than non-aqueous electrolyte secondary batteries for consumer use used in mobile phones and laptop computers. Long cycle life is strictly required.
  • Increasing the amount of the aqueous binder in the negative electrode active material layer to improve vibration resistance improves the binding property of the negative electrode active material layer and increases the peel strength between the negative electrode current collector and the negative electrode active material layer. be able to.
  • the amount of the aqueous binder is excessively large, the electrode becomes hard and brittle, and the vibration resistance is lowered.
  • a large residual stress is likely to be generated due to expansion and contraction of the negative electrode active material layer accompanying charging / discharging of the battery, and the electrode may be deformed and destroyed.
  • the current collector easily follows the swelling / shrinkage of the negative electrode active material layer accompanying the charging / discharging of the battery, and the electrode is not easily deformed. Residual stress hardly occurs in the electrode. Further, by making the shape of the electrode close to a square, it is possible to easily escape stress to the periphery. Therefore, high peel strength between the negative electrode active material and the current collector can be obtained. Furthermore, by controlling the amount of the aqueous binder to a specific value, it is possible to suppress the breakage of the electrode while ensuring the binding force. As a result, a high-performance nonaqueous electrolyte secondary battery that can be applied as a battery for a vehicle that has a high negative electrode binding property and receives strong vibrations can be obtained.
  • non-aqueous electrolyte lithium ion secondary battery will be described as a preferred embodiment of the non-aqueous electrolyte secondary battery, but is not limited to the following embodiment.
  • the same elements are denoted by the same reference numerals, and redundant description is omitted.
  • the dimensional ratios in the drawings are exaggerated for convenience of explanation, and may be different from the actual ratios.
  • FIG. 1 is a schematic cross-sectional view schematically showing a basic configuration of a non-aqueous electrolyte lithium ion secondary battery (hereinafter also simply referred to as “stacked battery”) that is not a flat (stacked) bipolar type.
  • the stacked battery 10 of the present embodiment has a structure in which a substantially rectangular power generation element 21 in which a charge / discharge reaction actually proceeds is sealed inside a battery exterior material 29 that is an exterior body.
  • the power generation element 21 has a configuration in which a positive electrode, a separator 17, and a negative electrode are stacked.
  • the separator 17 contains a nonaqueous electrolyte (for example, a liquid electrolyte).
  • the positive electrode has a structure in which the positive electrode active material layers 15 are disposed on both surfaces of the positive electrode current collector 12.
  • the negative electrode has a structure in which the negative electrode active material layer 13 is disposed on both surfaces of the negative electrode current collector 11.
  • the negative electrode, the electrolyte layer, and the positive electrode are laminated in this order so that one positive electrode active material layer 15 and the negative electrode active material layer 13 adjacent thereto face each other with a separator 17 therebetween.
  • the adjacent positive electrode, electrolyte layer, and negative electrode constitute one unit cell layer 19. Therefore, it can be said that the stacked battery 10 shown in FIG. 1 has a configuration in which a plurality of single battery layers 19 are stacked and electrically connected in parallel.
  • the negative electrode active material layer 13 is arrange
  • the positive electrode current collector 12 and the negative electrode current collector 11 are each provided with a positive electrode current collector plate (tab) 27 and a negative electrode current collector plate (tab) 25 that are electrically connected to the respective electrodes (positive electrode and negative electrode). It has the structure led out of the battery exterior material 29 so that it may be pinched
  • the positive electrode current collector 27 and the negative electrode current collector 25 are ultrasonically welded to the positive electrode current collector 12 and the negative electrode current collector 11 of each electrode, respectively, via a positive electrode lead and a negative electrode lead (not shown) as necessary. Or resistance welding or the like.
  • FIG. 1 shows a flat battery (stacked battery) that is not a bipolar battery, but a positive electrode active material layer that is electrically coupled to one surface of the current collector and the opposite side of the current collector.
  • a bipolar battery including a bipolar electrode having a negative electrode active material layer electrically coupled to the surface.
  • one of the current collectors also serves as a positive electrode current collector and a negative electrode current collector.
  • the negative electrode is formed by forming a negative electrode active material layer on the surface of the negative electrode current collector.
  • the negative electrode used in the nonaqueous electrolyte secondary battery of the present embodiment has a negative electrode active material layer 13 on the surface of the negative electrode current collector 11 having a long side with a length a and a short side with a length b. It is formed in a rectangular shape having
  • the length b of the short side of each negative electrode active material layer is preferably 100 mm or more.
  • the battery according to the present embodiment ensures the peel strength against the residual stress accompanying expansion / contraction of the negative electrode active material layer accompanying charging / discharging of the battery, but the electrode is more susceptible to bending as the size of the electrode increases. Therefore, a particularly remarkable effect can be obtained in a large battery.
  • the upper limit of the short side length of the negative electrode active material layer is not particularly limited, but is usually 400 mm or less.
  • the length ratio (a / b) between the long side and the short side of each negative electrode active material layer is 1 to 1.25. If the ratio of the length of the long side to the short side is larger than 1.25, residual stress is generated in the long axis direction, and the binding property can be lowered. This also increases the cell resistance and can reduce the initial capacity of the battery.
  • the ratio of the long side to the short side of the negative electrode active material layer is preferably close to 1, preferably 1 to 1.1, more preferably 1 to 1.05.
  • the Young's modulus of each negative electrode is preferably 1.0 to 1.4 GPa, more preferably 1.1 to 1.3 GPa.
  • the Young's modulus of the negative electrode can be controlled by adjusting the type or amount of the aqueous binder. For example, by using a binder having many crosslinking points such as a rubber-based binder, it can be restored even when the negative electrode is extended by an external force.
  • the Young's modulus of the negative electrode can be determined by the method described in the examples.
  • the 90 ° peel strength from the negative electrode active material layer of the negative electrode current collector in each negative electrode is 30 N / m or more, more preferably 50 N / m or more. If it is the said range, the battery which has high vibration resistance will be obtained, and it can be used suitably as a battery for vehicles which receives a strong vibration.
  • the upper limit of 90 degree peeling strength in a negative electrode is not specifically limited, For example, it is 70 N / m or less.
  • the negative electrode active material layer includes a negative electrode active material.
  • the negative electrode active material include carbon materials such as graphite (graphite), soft carbon, and hard carbon, lithium-transition metal composite oxides (for example, Li 4 Ti 5 O 12 ), metal materials, lithium alloy negative electrode materials, and the like. Is mentioned. In some cases, two or more negative electrode active materials may be used in combination. Preferably, from the viewpoint of capacity and output characteristics, a carbon material or a lithium-transition metal composite oxide is used as the negative electrode active material. Of course, negative electrode active materials other than those described above may be used.
  • the average particle diameter of each active material contained in the negative electrode active material layer is not particularly limited, but is preferably 1 to 100 ⁇ m, more preferably 1 to 30 ⁇ m from the viewpoint of high output.
  • the negative electrode active material layer contains at least an aqueous binder.
  • water-based binders can be greatly reduced in capital investment on the production line and reduced environmental load because it is water vapor that occurs during drying. There is an advantage. Further, it is not necessary to use an expensive organic solvent to dissolve or disperse the binder, and the cost can be reduced.
  • the amount of the aqueous binder contained in the negative electrode active material layer of the battery of this embodiment is 2 to 4% by mass with respect to the total mass of the negative electrode active material layer.
  • the amount of the aqueous binder is less than 2% by mass, sufficient binding properties cannot be ensured, and thus high vibration resistance cannot be obtained. If it exceeds 4% by mass, especially when a crosslinkable polymer binder such as SBR is included, the entire electrode becomes hard and brittle, and vibration resistance decreases. Moreover, battery performance will fall. More preferably, the amount of the aqueous binder in the negative electrode active material layer is 2.5 to 3.5% by mass.
  • the content of the aqueous binder is preferably 80 to 100% by mass, preferably 90 to 100% by mass, and preferably 100% by mass.
  • the binder other than the water-based binder include binders used in the following positive electrode active material layer.
  • the water-based binder refers to a binder using water as a solvent or a dispersion medium, and specifically includes a thermoplastic resin, a polymer having rubber elasticity, a water-soluble polymer, or a mixture thereof.
  • the binder using water as a dispersion medium refers to a polymer that includes all expressed as latex or emulsion and is emulsified or suspended in water.
  • kind a polymer latex that is emulsion-polymerized in a system that self-emulsifies.
  • water-based binders include styrene polymers (styrene-butadiene rubber, styrene-vinyl acetate copolymer, styrene-acrylic copolymer, etc.), acrylonitrile-butadiene rubber, methyl methacrylate-butadiene rubber, ) Acrylic polymers (polyethyl acrylate, polyethyl methacrylate, polypropyl acrylate, polymethyl methacrylate (methyl methacrylate rubber), polypropyl methacrylate, polyisopropyl acrylate, polyisopropyl methacrylate, polybutyl acrylate, polybutyl methacrylate, polyhexyl acrylate , Polyhexyl methacrylate, polyethylhexyl acrylate, polyethylhexyl methacrylate, polylauryl acrylate, polylauryl meta Acrylate, etc.), polytyren
  • the aqueous binder may contain at least one rubber binder selected from the group consisting of styrene-butadiene rubber, acrylonitrile-butadiene rubber, methyl methacrylate-butadiene rubber, and methyl methacrylate rubber from the viewpoint of binding properties. preferable. Furthermore, it is preferable that the water-based binder contains styrene-butadiene rubber because of good binding properties.
  • Water-soluble polymers suitable for use in combination with styrene-butadiene rubber include polyvinyl alcohol and modified products thereof, starch and modified products thereof, cellulose derivatives (such as carboxymethyl cellulose, methyl cellulose, hydroxyethyl cellulose, and salts thereof), polyvinyl Examples include pyrrolidone, polyacrylic acid (salt), or polyethylene glycol.
  • the cellulose derivative can be preferably used because it provides an appropriate thickening effect in the negative electrode manufacturing process and can form a flat and smooth negative electrode active material layer.
  • the amount of the rubber-based binder contained in the negative electrode active material layer of the battery of the present embodiment is not particularly limited, but is preferably 0.5 to 3.5% by mass with respect to the total mass of the negative electrode active material layer, and more The amount is preferably 1.5 to 2.5% by mass.
  • the content of the rubber-based binder is 1% by mass or more, high binding properties can be obtained in the negative electrode active material layer, and high peel strength between the negative electrode current collector and the negative electrode active material layer can be obtained.
  • the quantity of a rubber-type binder is 4 mass% or less, it can prevent that an electrode will become hard and brittle.
  • the amount of the water-soluble polymer contained in the negative electrode active material layer of the battery of the present embodiment is not particularly limited, and is, for example, 0.5 to 3.5% by mass with respect to the total mass of the negative electrode active material layer. More preferably, it is 1 to 2% by mass. If the content of the cellulose derivative is within the above range, an excellent thickening effect can be obtained in the negative electrode production process, and the viscosity of the negative electrode active material slurry can be appropriately adjusted.
  • the negative electrode active material layer further includes other additives such as a conductive additive, an electrolyte (polymer matrix, ion conductive polymer, electrolytic solution, etc.), and a lithium salt for improving ion conductivity, as necessary.
  • the conductive assistant means an additive blended to improve the conductivity of the positive electrode active material layer or the negative electrode active material layer.
  • the conductive auxiliary agent include carbon materials such as carbon black such as acetylene black, graphite, and carbon fiber.
  • electrolyte salt examples include Li (C 2 F 5 SO 2 ) 2 N, LiPF 6 , LiBF 4 , LiClO 4 , LiAsF 6 , LiCF 3 SO 3 and the like.
  • Examples of the ion conductive polymer include polyethylene oxide (PEO) and polypropylene oxide (PPO) polymers.
  • the compounding ratio of the components contained in the negative electrode active material layer other than the aqueous binder can be adjusted by appropriately referring to known knowledge about the lithium ion secondary battery.
  • the density of the negative electrode active material layer is not particularly limited, but is preferably 1.4 to 1.6 g / cm 3 .
  • the density of the negative electrode active material layer is 1.4 g / cm 3 or more, the peel strength of the negative electrode is improved, so that the resistance is hardly increased and a high-performance battery can be obtained.
  • the density of the negative electrode active material layer is 1.6 g / cm 3 or less, sufficient communication of the negative electrode active material can be obtained, and the electrolyte solution can easily penetrate, so that battery performance such as initial capacity and cycle durability can be obtained. Can be improved.
  • the density of the negative electrode active material layer is preferably 1.45 to 1.55 g / cm 3 because the effects of the present invention are more exhibited.
  • the density of the negative electrode active material layer represents the mass of the active material layer per unit volume. Specifically, after removing the negative electrode active material layer from the battery, removing the solvent, etc. present in the electrolyte, the active material layer volume is obtained from the long side, short side, and height, and the weight of the active material layer is measured. Later, it can be determined by dividing the weight by the volume.
  • examples of the metal include aluminum, nickel, iron, stainless steel, titanium, copper, and other alloys.
  • a clad material of nickel and aluminum, a clad material of copper and aluminum, or a plating material of a combination of these metals can be preferably used.
  • covered on the metal surface may be sufficient.
  • aluminum, stainless steel, and copper are preferable from the viewpoints of electronic conductivity and battery operating potential.
  • the size of the current collector is determined according to the intended use of the battery. For example, if it is used for a large battery that requires a high energy density, a current collector having a large area is used. In the battery of this embodiment, preferably, since the length of the short side of the negative electrode active material layer is 100 mm or more, a current collector whose length of the short side is 100 mm or more is used. There is no particular limitation on the thickness of the current collector. The thickness of the current collector is usually about 1 to 100 ⁇ m.
  • the manufacturing method of the negative electrode is not particularly limited.
  • a negative electrode active material slurry is prepared by mixing a component constituting a negative electrode active material layer containing a negative electrode active material and an aqueous binder and an aqueous solvent that is a slurry viscosity adjusting solvent, and applying this to the surface of the current collector. Thereafter, a method of drying and pressing can be used.
  • the aqueous solvent as the slurry viscosity adjusting solvent is not particularly limited, and a conventionally known aqueous solvent can be used.
  • a conventionally known aqueous solvent can be used.
  • water pure water, ultrapure water, distilled water, ion exchange water, ground water, well water, tap water (tap water), etc.
  • a mixed solvent of water and alcohol eg, ethyl alcohol, methyl alcohol, isopropyl alcohol, etc.
  • Etc. eg, ethyl alcohol, methyl alcohol, isopropyl alcohol, etc.
  • a conventionally well-known aqueous solvent can be selected suitably and used as long as the effect of this embodiment is not impaired.
  • the blending amount of the aqueous solvent is not particularly limited, and an appropriate amount may be blended so that the negative electrode active material slurry is within a desired viscosity range.
  • the basis weight when applying the negative electrode active material slurry to the current collector is not particularly limited, but is preferably 0.5 to 20 g / m 2 , more preferably 1 to 10 g / m 2 . If it is the said range, the negative electrode active material layer which has suitable thickness can be obtained.
  • the coating method is not particularly limited, and examples thereof include a knife coater method, a gravure coater method, a screen printing method, a wire bar method, a die coater method, a reverse roll coater method, an ink jet method, a spray method, and a roll coater method.
  • the method for drying the negative electrode active material slurry after coating is not particularly limited, and for example, a method such as warm air drying may be used.
  • the drying temperature is, for example, 30 to 100 ° C.
  • the drying time is, for example, 2 seconds to 1 hour.
  • the thickness of the negative electrode active material layer obtained in this manner is not particularly limited, but is 2 to 100 ⁇ m, for example.
  • the positive electrode used in the nonaqueous electrolyte secondary battery of the present embodiment has a positive electrode active material layer formed on the surface of a positive electrode current collector.
  • the shape and size of the positive electrode are not particularly limited, but the positive electrode active material layer is preferably formed in a shape having a short side of 100 mm or more and an aspect ratio of 1 to 1.25.
  • the positive electrode active material layer contains a positive electrode active material and, if necessary, other materials such as a conductive additive, a binder, an electrolyte (polymer matrix, ion conductive polymer, electrolyte, etc.), a lithium salt for increasing ion conductivity, and the like. Further includes an additive.
  • the positive electrode active material layer includes a positive electrode active material.
  • the positive electrode active material include LiMn 2 O 4 , LiCoO 2 , LiNiO 2 , Li (Ni—Mn—Co) O 2, and lithium-- such as those in which some of these transition metals are substituted with other elements.
  • Examples include transition metal composite oxides, lithium-transition metal phosphate compounds, and lithium-transition metal sulfate compounds.
  • two or more positive electrode active materials may be used in combination.
  • a lithium-transition metal composite oxide is used as the positive electrode active material.
  • NMC composite oxide Li (Ni—Mn—Co) O 2 and those in which some of these transition metals are substituted with other elements (hereinafter also simply referred to as “NMC composite oxide”) are used.
  • the NMC composite oxide has a layered crystal structure in which a lithium atomic layer and a transition metal (Mn, Ni, and Co are arranged in order) are stacked alternately via an oxygen atomic layer.
  • One Li atom is contained, and the amount of Li that can be taken out is twice that of the spinel lithium manganese oxide, that is, the supply capacity is doubled, so that a high capacity can be obtained.
  • the NMC composite oxide includes a composite oxide in which a part of the transition metal element is substituted with another metal element.
  • Other elements in that case include Ti, Zr, Nb, W, P, Al, Mg, V, Ca, Sr, Cr, Fe, B, Ga, In, Si, Mo, Y, Sn, V, Cu , Ag, Zn, etc., preferably Ti, Zr, Nb, W, P, Al, Mg, V, Ca, Sr, Cr, more preferably Ti, Zr, P, Al, Mg, From the viewpoint of improving cycle characteristics, Ti, Zr, Al, Mg, and Cr are more preferable.
  • a represents the atomic ratio of Li
  • b represents the atomic ratio of Ni
  • c represents the atomic ratio of Mn
  • d represents the atomic ratio of Co
  • x represents the atomic ratio of M. Represents. From the viewpoint of cycle characteristics, it is preferable that 0.4 ⁇ b ⁇ 0.6 in the general formula (1).
  • the composition of each element can be measured by, for example, inductively coupled plasma (ICP) emission spectrometry.
  • ICP inductively coupled plasma
  • Ni nickel
  • Co cobalt
  • Mn manganese
  • Ti or the like partially replaces the transition metal in the crystal lattice. From the viewpoint of cycle characteristics, it is preferable that a part of the transition element is substituted with another metal element, and it is particularly preferable that 0 ⁇ x ⁇ 0.3 in the general formula (1). Since at least one selected from the group consisting of Ti, Zr, Nb, W, P, Al, Mg, V, Ca, Sr, and Cr is dissolved, the crystal structure is stabilized. It is considered that the battery capacity can be prevented from decreasing even if the above is repeated, and that excellent cycle characteristics can be realized.
  • b, c and d are 0.44 ⁇ b ⁇ 0.51, 0.27 ⁇ c ⁇ 0.31, 0.19 ⁇ d ⁇ 0.26. It is preferable that it is excellent in balance between capacity and durability.
  • positive electrode active materials other than those described above may be used.
  • the average particle diameter of the positive electrode active material contained in the positive electrode active material layer is not particularly limited, but is preferably 1 to 100 ⁇ m, more preferably 1 to 20 ⁇ m from the viewpoint of increasing the output.
  • a binder used for a positive electrode active material layer For example, the following materials are mentioned. Polyethylene, polypropylene, polyethylene terephthalate (PET), polyether nitrile, polyacrylonitrile, polyimide, polyamide, cellulose, carboxymethyl cellulose (CMC) and its salts, ethylene-vinyl acetate copolymer, polyvinyl chloride, styrene-butadiene rubber (SBR) ), Isoprene rubber, butadiene rubber, ethylene / propylene rubber, ethylene / propylene / diene copolymer, styrene / butadiene / styrene block copolymer and hydrogenated product thereof, styrene / isoprene / styrene block copolymer and hydrogenated product thereof.
  • Thermoplastic polymers such as products, polyvinylidene fluoride (PVdF), polyt
  • the amount of the binder contained in the positive electrode active material layer is not particularly limited as long as it is an amount capable of binding the active material, but preferably 0.5 to 15% by mass with respect to the active material layer. More preferably, it is 1 to 10% by mass.
  • additives other than the binder the same additives as those in the negative electrode active material layer column can be used.
  • the separator has a function of holding an electrolyte and ensuring lithium ion conductivity between the positive electrode and the negative electrode, and a function as a partition wall between the positive electrode and the negative electrode.
  • Examples of the form of the separator include a separator made of a porous sheet made of a polymer or fiber that absorbs and holds the electrolyte and a nonwoven fabric separator.
  • the separator preferably has a porosity of 40 to 65%.
  • a microporous (microporous film) can be used as the separator of the porous sheet made of polymer or fiber.
  • the porous sheet made of the polymer or fiber include polyolefins such as polyethylene (PE) and polypropylene (PP); a laminate in which a plurality of these are laminated (for example, three layers of PP / PE / PP) And a microporous (microporous membrane) separator made of a hydrocarbon resin such as polyimide, aramid, polyvinylidene fluoride-hexafluoropropylene (PVdF-HFP), glass fiber, and the like.
  • PE polyethylene
  • PP polypropylene
  • a microporous (microporous membrane) separator made of a hydrocarbon resin such as polyimide, aramid, polyvinylidene fluoride-hexafluoropropylene (PVdF-HFP), glass fiber, and the like.
  • the thickness of the microporous (microporous membrane) separator cannot be uniquely defined because it varies depending on the intended use. For example, in applications such as secondary batteries for driving motors such as electric vehicles (EV), hybrid electric vehicles (HEV), and fuel cell vehicles (FCV), it is 4 to 60 ⁇ m in a single layer or multiple layers. Is desirable.
  • the fine pore diameter of the microporous (microporous membrane) separator is desirably 1 ⁇ m or less (usually a pore diameter of about several tens of nm).
  • nonwoven fabric separator cotton, rayon, acetate, nylon, polyester; polyolefins such as PP and PE; conventionally known ones such as polyimide and aramid are used alone or in combination.
  • the bulk density of the nonwoven fabric is not particularly limited as long as sufficient battery characteristics can be obtained by the impregnated polymer gel electrolyte.
  • the thickness of the nonwoven fabric separator may be the same as that of the electrolyte layer, and is preferably 5 to 200 ⁇ m, particularly preferably 10 to 100 ⁇ m.
  • the battery according to the present embodiment can form a single battery layer in the battery 10 shown in FIG. 1 by forming an electrolyte layer by holding an electrolyte in the separator portion.
  • an electrolyte layer by holding an electrolyte in the separator portion.
  • Polymer electrolytes such as a liquid electrolyte and a polymer gel electrolyte, can be used suitably.
  • the means for holding the electrolyte in the separator portion is not particularly limited, and for example, means such as impregnation, coating, and spraying can be applied.
  • the liquid electrolyte functions as a lithium ion carrier.
  • the liquid electrolyte constituting the electrolytic solution layer has a form in which a lithium salt as a supporting salt is dissolved in an organic solvent as a plasticizer.
  • organic solvent include carbonates such as ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), and ethyl methyl carbonate.
  • EC ethylene carbonate
  • PC propylene carbonate
  • DMC dimethyl carbonate
  • DEC diethyl carbonate
  • ethyl methyl carbonate ethyl methyl carbonate.
  • Li (CF 3 SO 2) 2 N Li (C 2 F 5 SO 2) 2 N, LiPF 6, LiBF 4, LiClO 4, LiAsF 6, LiTaF such 6, LiCF 3 SO 3
  • a compound that can be added to the active material layer of the electrode can be similarly employed.
  • the liquid electrolyte may further contain additives other than the components described above.
  • additives include, for example, vinylene carbonate, methyl vinylene carbonate, dimethyl vinylene carbonate, phenyl vinylene carbonate, diphenyl vinylene carbonate, ethyl vinylene carbonate, diethyl vinylene carbonate, vinyl ethylene carbonate, 1,2-divinyl ethylene carbonate.
  • vinylene carbonate, methyl vinylene carbonate, and vinyl ethylene carbonate are preferable, and vinylene carbonate and vinyl ethylene carbonate are more preferable.
  • These cyclic carbonates may be used alone or in combination of two or more.
  • a gel polymer electrolyte (gel electrolyte) containing an electrolytic solution can be preferably used.
  • the gel polymer electrolyte has a configuration in which the above liquid electrolyte is injected into a matrix polymer (host polymer) made of an ion conductive polymer.
  • a gel polymer electrolyte as the electrolyte is superior in that the fluidity of the electrolyte is lost and the ion conductivity between the layers is easily cut off.
  • the ion conductive polymer used as the matrix polymer (host polymer) include polyethylene oxide (PEO), polypropylene oxide (PPO), and copolymers thereof. In such polyalkylene oxide polymers, electrolyte salts such as lithium salts can be well dissolved.
  • the matrix polymer of gel electrolyte can express excellent mechanical strength by forming a crosslinked structure.
  • thermal polymerization, ultraviolet polymerization, radiation polymerization, electron beam polymerization, etc. are performed on a polymerizable polymer (for example, PEO or PPO) for forming a polymer electrolyte using an appropriate polymerization initiator.
  • a polymerization treatment may be performed.
  • the material which comprises a current collector plate (25, 27) is not restrict
  • a constituent material of the current collector plate for example, metal materials such as aluminum, copper, titanium, nickel, stainless steel (SUS), and alloys thereof are preferable. From the viewpoint of light weight, corrosion resistance, and high conductivity, aluminum and copper are more preferable, and aluminum is particularly preferable.
  • the same material may be used for the positive electrode current collecting plate 27 and the negative electrode current collecting plate 25, and different materials may be used.
  • the current collectors 11 and 12 and the current collector plates (25 and 27) may be electrically connected via a positive electrode lead or a negative electrode lead.
  • a constituent material of the positive electrode and the negative electrode lead materials used in known lithium ion secondary batteries can be similarly employed.
  • heat-shrinkable heat-shrinkable parts are removed from the exterior so that they do not affect products (for example, automobile parts, especially electronic devices) by touching peripheral devices or wiring and causing leakage. It is preferable to coat with a tube or the like.
  • the battery outer case 29 a known metal can case can be used, and a bag-like case using a laminate film containing aluminum that can cover the power generation element can be used.
  • a laminate film having a three-layer structure in which PP, aluminum, and nylon are laminated in this order can be used as the laminate film, but the laminate film is not limited thereto.
  • a laminate film is desirable from the viewpoint that it is excellent in high output and cooling performance, and can be suitably used for a battery for large equipment for EV and HEV.
  • the negative electrode active material layer is preferably rectangular, and the length of the short side of the rectangle is preferably 100 mm or more.
  • the length of the short side of the negative electrode active material layer refers to the side having the shortest length among the electrodes.
  • the upper limit of the length of the short side of the battery structure is not particularly limited, but is usually 250 mm or less.
  • the value of the ratio of the battery area to the rated capacity (the maximum value of the projected area of the battery including the battery outer casing) is 5 cm 2 / Ah or more, and the rated capacity is In a battery having a capacity of 3 Ah or more, the battery area per unit capacity is large, so that the battery is easily affected by residual stress accompanying expansion / contraction of the negative electrode active material layer accompanying charge / discharge of the battery.
  • the nonaqueous electrolyte secondary battery according to the present embodiment is a battery having a large size as described above from the viewpoint that the merit due to the expression of the effects of the present invention is greater.
  • the aspect ratio of the rectangular electrode is preferably 1 to 1.25, more preferably 1 to 1.1.
  • the electrode aspect ratio is defined as the aspect ratio of the rectangular positive electrode active material layer.
  • the group pressure applied to the power generation element of the flat plate type battery is preferably 0.07 to 0.7 kgf / cm 2 (6.86 to 68.6 kPa).
  • the group pressure applied to the power generation element of the flat plate type battery is preferably 0.07 to 0.7 kgf / cm 2 (6.86 to 68.6 kPa).
  • the group pressure applied to the power generation element is 0.1 to 0.7 kgf / cm 2 (9.80 to 68.6 kPa).
  • the group pressure refers to an external force applied to the power generation element, and the group pressure applied to the power generation element can be easily measured using a film-type pressure distribution measuring system. A value measured using a film-type pressure distribution measuring system is adopted.
  • the control of the group pressure is not particularly limited, but can be controlled by applying an external force physically or directly to the power generation element and controlling the external force.
  • an external force it is preferable to use a pressure member that applies pressure to the exterior body.
  • FIG. 3A is a plan view of a non-aqueous electrolyte secondary battery which is another preferred embodiment of the present invention
  • FIG. 3B is an arrow view from A in FIG. 3A.
  • the exterior body 1 enclosing the power generation element has a rectangular flat shape, and an electrode tab 4 for taking out electric power is drawn out from the side portion.
  • the power generation element is wrapped by a battery outer package, and the periphery thereof is heat-sealed.
  • the power generation element is sealed with the electrode tab 4 pulled out.
  • the power generation element corresponds to the power generation element 21 of the lithium ion secondary battery 10 shown in FIG. 1 described above.
  • FIG. 1 the power generation element 21 of the lithium ion secondary battery 10 shown in FIG. 1 described above.
  • 2 is a SUS plate that is a pressure member
  • 3 is a fixing jig that is a fixing member
  • 4 is an electrode tab (negative electrode tab or positive electrode tab).
  • the pressurizing member is disposed for the purpose of controlling the group pressure applied to the power generation element to be 0.07 to 0.7 kgf / cm 2 .
  • the pressure member include rubber materials such as urethane rubber sheets, metal plates such as aluminum and SUS, resin films such as PP, and heat resistant resin sheets such as polyimide.
  • the pressure member can continuously apply a constant pressure to the power generation element, it is preferable to further include a fixing member for fixing the pressure member. Further, the group pressure applied to the power generation element can be easily controlled by adjusting the fixing of the fixing jig to the pressing member.
  • the tab removal shown in FIG. 3 is not particularly limited.
  • the positive electrode tab and the negative electrode tab may be pulled out from both sides, or the positive electrode tab and the negative electrode tab may be divided into a plurality of parts and taken out from each side. It is not a thing.
  • said nonaqueous electrolyte secondary battery can be manufactured with a conventionally well-known manufacturing method.
  • the assembled battery is configured by connecting a plurality of batteries. Specifically, at least two or more are used, and are configured by serialization, parallelization, or both. Capacitance and voltage can be freely adjusted by paralleling in series.
  • a small assembled battery that can be attached and detached by connecting a plurality of batteries in series or in parallel. Then, a plurality of small assembled batteries that can be attached and detached are connected in series or in parallel to provide a large capacity and large capacity suitable for vehicle drive power supplies and auxiliary power supplies that require high volume energy density and high volume output density.
  • An assembled battery having an output can also be formed. How many batteries are connected to make an assembled battery, and how many small assembled batteries are stacked to make a large-capacity assembled battery depends on the battery capacity of the mounted vehicle (electric vehicle) It may be determined according to the output.
  • the non-aqueous electrolyte secondary battery or an assembled battery using the non-aqueous electrolyte battery has excellent output characteristics, maintains a discharge capacity even after long-term use, and has good cycle characteristics.
  • Vehicle applications such as electric vehicles, hybrid electric vehicles, fuel cell vehicles, and hybrid fuel cell vehicles require higher capacity, larger size, and longer life than electric and portable electronic devices. . Therefore, the non-aqueous electrolyte secondary battery or the assembled battery using the non-aqueous electrolyte battery can be suitably used as a vehicle power source, for example, a vehicle driving power source or an auxiliary power source.
  • a battery or an assembled battery formed by combining a plurality of these batteries can be mounted on the vehicle.
  • a plug-in hybrid electric vehicle having a long EV travel distance or an electric vehicle having a long charge travel distance can be configured.
  • a car a hybrid car, a fuel cell car, an electric car (four-wheeled vehicles (passenger cars, trucks, buses, commercial vehicles, light cars, etc.)
  • the application is not limited to automobiles.
  • it can be applied to various power sources for moving vehicles such as other vehicles, for example, trains, and power sources for mounting such as uninterruptible power supplies. It is also possible to use as.
  • a solid content consisting of 85% by mass of LiMn 2 O 4 (average particle size: 15 ⁇ m) as a positive electrode active material, 5% by mass of acetylene black as a conductive assistant, and 10% by mass of PVdF as a binder was prepared.
  • NMP N-methyl-2-pyrrolidone
  • the coating amount on one side was 25 mg / cm 2 .
  • the negative electrode slurry was applied to both sides of a copper foil (200 mm ⁇ 200 mm, thickness 20 ⁇ m) as a current collector and dried.
  • the coating amount on one side was 8 mg / cm 2 .
  • the density of the obtained negative electrode active material layer was 1.45 g / cm 3 .
  • Each of the positive electrode and the negative electrode obtained above was cut into a predetermined size.
  • the positive electrode and the negative electrode were laminated via a separator (microporous polyethylene film, thickness: 15 ⁇ m) to produce a 15-layer laminate.
  • a tab is welded to each of the positive electrode and the negative electrode, the laminate is encased in an exterior material made of an aluminum laminate film, one side of the laminate is opened, an electrolyte is injected from one side, and then the vacuum is drawn to provide an electrolyte.
  • One side into which was injected was sealed.
  • the internal resistance of the battery was measured as follows.
  • the DC resistance was measured when charged for 30 minutes with a constant current (current: 220 mA (1 CA)). The DC resistance was measured by discharging for 30 seconds, and the resistance value was calculated from the cell voltage change ⁇ V and the current value.
  • the peel strength was measured in accordance with JIS K 6854-1 (Adhesive-Peeling peel strength test method-Part 1: 90 degree peel). As the sample, the negative electrode after the negative electrode active material layer was applied, dried and pressed was cut into a size of 20 mm ⁇ 100 mm and used.
  • Example 1 A negative electrode active material layer was prepared by changing the ratio of the length of the long side to the short side (long side / short side) of the negative electrode active material layer as shown in Table 1 below, and producing a battery from the negative electrode current collector in the negative electrode. 90 ° peel strength and DC resistance were measured. The results are shown in Table 1 below and FIG. The values of 90 ° peel strength and direct current resistance were expressed as relative values when the values obtained in Example 1-1 and Example 1-3 were set to 1, respectively.
  • the negative electrode active material layer of the battery produced in Example 1 was prepared so that the length of the short side and the long side was the ratio of the long side / short side shown in Table 1 below.
  • the content of the aqueous binder, the density of the negative electrode active material layer, and the Young's modulus of the negative electrode were as follows.
  • Table 1 shows the rated capacity (cell capacity, initial capacity) of the battery thus manufactured, and the ratio of the battery area (projected area of the battery including the battery outer package) to the rated capacity.
  • Example 2 Batteries were prepared by changing the aqueous binder content of the negative electrode active material layer as follows, and 90 ° peel strength, DC resistance, and initial capacity were measured. In either case, the ratio of SBR: CMC was 2: 1 (mass ratio) in the aqueous binder. The results are shown in Table 2 below and FIG. The values of 90 ° peel strength and initial capacity were expressed as relative values when the value obtained in Example 2-2 was 1, respectively. The value of the direct current resistance was expressed as a relative value when the value obtained in Example 2-6 was 1.
  • the lengths of the long and short sides of the negative electrode active material layer of the battery produced in Example 2 were as follows. Other conditions were the same.
  • negative electrode active material layer 200 ⁇ 200 mm
  • Binder content in negative electrode active material 3.0% by mass
  • Active material layer density 1.45 g / cm 3
  • Young's modulus of the negative electrode 1.2 GPa.
  • Table 2 shows the rated capacity (cell capacity, initial capacity) of the battery thus manufactured, and the ratio of the battery area (projected area of the battery including the battery outer package) to the rated capacity.
  • Example 3 Batteries were prepared by changing the Young's modulus of the negative electrode as follows, and 90 ° peel strength, DC resistance, and initial capacity were measured. The results are shown in Table 3 below and FIG. The values of 90 ° peel strength and initial capacity were expressed as relative values when the value obtained in Example 3-2 was 1, respectively. The value of DC resistance was expressed as a relative value.
  • the lengths of the long and short sides of the negative electrode active material layer of the battery produced in Example 3, the density of the negative electrode active material layer, and the Young's modulus of the negative electrode were as follows. The Young's modulus was adjusted by changing the cross-sectional area of the electrode.
  • Table 3 shows the rated capacity (cell capacity, initial capacity) of the battery thus manufactured, and the ratio of the battery area (projected area of the battery including the battery outer package) to the rated capacity.
  • Example 4 Batteries were prepared by changing the density of the negative electrode as follows, and 90 ° peel strength, DC resistance, and initial capacity were measured. The results are shown in Table 4 below and FIG. The values of 90 ° peel strength, DC resistance, and initial capacity are expressed as relative values when the values obtained in Example 4-4, Example 4-5, and Example 4-2 are set to 1. did.
  • the lengths of the long and short sides of the negative electrode active material layer of the battery produced in Example 4 were as follows.
  • Table 4 shows the rated capacity (cell capacity, initial capacity) of the battery thus manufactured, and the ratio of the battery area (projected area of the battery including the battery outer package) to the rated capacity.

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